WO2009118124A1 - Procédé de réduction d'oxygène électrolytique - Google Patents
Procédé de réduction d'oxygène électrolytique Download PDFInfo
- Publication number
- WO2009118124A1 WO2009118124A1 PCT/EP2009/002028 EP2009002028W WO2009118124A1 WO 2009118124 A1 WO2009118124 A1 WO 2009118124A1 EP 2009002028 W EP2009002028 W EP 2009002028W WO 2009118124 A1 WO2009118124 A1 WO 2009118124A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- catalyst
- oxygen
- nitrogen
- chloride
- chlorine
- Prior art date
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/24—Halogens or compounds thereof
- C25B1/26—Chlorine; Compounds thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/18—Carbon
- B01J21/185—Carbon nanotubes
Definitions
- the invention relates to a process for oxygen reduction in aqueous chlorine and / or chloride-containing solutions in the presence of a catalyst comprising nitrogen-doped carbon nanotubes.
- catalysts for the reduction of oxygen are often used. In particular, this should reduce the energy costs of the process.
- catalysts include noble metals or compounds comprising noble metals such as platinum and compounds comprising platinum, so that the processes are generally very costly.
- a catalyst comprising rhodium sulphide (RhS x) disclosed as the essential catalytic active component can be reduced in aqueous, chloride containing solutions with the oxygen.
- RhS x rhodium sulphide
- US Pat. No. 6,149,782 discloses that the use of rhodium sulphide is advantageous because the omission of pure noble metals (in particular platinum) has, inter alia, the consequence that dissolution of the catalytically active component of the catalyst only occurs to a greatly reduced extent.
- leaching of the catalytically active component rhodium sulfide can also not be completely prevented, since rhodium and its compounds with chlorine form stable salts and / or complexes which are washed out to a small extent from the catalyst, so that it depleted of catalytically active material and thereby inactivated.
- the inactivated catalyst would thus have to be exchanged at regular intervals, with the result that the disadvantages of rhodium set out above render the process economically unattractive.
- catalytically active components which can be used in catalysts for the reduction of oxygen in aqueous solution containing chlorine and / or chloride.
- rhodium and platinum, iridium, rhenium, ruthenium and palladium, their sulfides and oxides, as well as mixed phases, in particular with molybdenum and / or selenium are also disclosed as possible catalytically active components.
- a combination of materials whose catalytic effect does not rely on noble or transition metals is not disclosed. It is also taught that it is advantageous not to bring hydrochloric acid in contact with the catalyst, as this prevents corrosive attack on the catalytically active components disclosed. Ideally, contact of chlorides and / or chlorine with the catalytically active component should be completely inhibited.
- the object is therefore to provide a method for oxygen reduction in aqueous solutions containing chlorine and / or chloride, which dispenses with the use of expensive noble and / or transition metals as the essential catalytically active component, the none Tendency to hydrogen generation, as well as no need to renew the catalytically active component, due to their consumption or inactivation, and which downsized the necessary cell voltage comparable far as it would in the case of a process, if no aqueous chlorine and / or chloride-containing solutions present would.
- aqueous solutions containing chlorine and / or chloride denote all solutions whose solvent is water and which contains molecular chlorine in dissolved or gaseous form and / or chloride, hypochlorite and / or chlorate and / or perchlorate. Include ions.
- Non-limiting examples are aqueous solutions of salts comprising chloride ions, hypochlorite and / or chlorate and / or perchlorate ions, such as NaCl, NaOCl, MgCl 2 , etc. with dissolved or gaseous molecular chlorine, but also acids which are soluble in water or miscible with it, such as H 2 SO 4 , HCl with dissolved or gaseous molecular chlorine.
- Particularly preferred are aqueous solutions of HCl with molecular chlorine dissolved therein.
- the concentration is usually 0.1-37% by weight of HCl, preferably 0.5-37% by weight of HCl.
- the chlorine- and / or chloride-containing solutions according to the invention may also comprise traces of impurities, without the process according to the invention being thereby hindered in its feasibility.
- Traces refer to concentrations of less than 1000 ppm in the context of the present invention.
- Possible impurities are e.g. organic contaminants such as alcohols miscible with water in the specified concentration or soluble in water.
- Examples of non-conclusive examples include methanol, ethanol, 1-propanol, 2-propanol, 1,2-propanediol, etc.
- Oxygen-comprising components in the context of the present invention designate all substances which comprise oxygen, the oxygen in the component being present in an oxidation state greater than -2.
- Examples of non-exhaustive examples are molecular oxygen and hydrogen peroxide.
- the component comprising oxygen may be dissolved in the aqueous solution or in gaseous form.
- the oxygen-comprising component is molecular oxygen.
- Particularly preferred is the oxygen comprising Component molecular oxygen that is dissolved in the aqueous solution.
- Catalyst in connection with the present invention denotes all substances or substance mixtures which comprise at least one catalytically active component which reduce the cell voltage of a half-cell comprising the electrochemical equilibrium according to formula (I):
- the catalysts used in the process according to the invention are characterized by a proportion of nitrogen-doped carbon nanotubes as the catalytically active component.
- the proportion of nitrogen-doped carbon nanotubes on the catalyst without an optional polymeric binder is usually at least 30% by weight. A proportion of at least 50% by weight is preferred.
- Nitrogen-doped carbon nanotubes in the context of the present invention, denote carbon nanotubes known to the person skilled in the art in their general form, which are characterized by fractions of nitrogen as part of the molecular structure of the carbon nanotubes. Methods by which these can be obtained can be found e.g. in German patent application DE 10 2007 062421.4, or in Paul H. Matter, Ling Zhang, Umit S. Ozkan, Journal of Catalysis 239 ("The role of nanostructure in nitrogen-containing carbonates"). 2006) 83-96.
- the nitrogen-doped carbon nanotubes used in the process according to the invention are usually carbon nanotubes which comprise at least 0.5% by weight of nitrogen.
- the nitrogen-doped carbon nanotubes comprise at least 1% by weight of nitrogen; particularly preferably at least 2% by weight of nitrogen.
- the nitrogen present in the nitrogen-doped carbon nanotubes according to the invention is incorporated in the graphitic layers and is preferably present as pyridinic nitrogen and / or as quaternary nitrogen and / or as nitroso nitrogen and / or as nitro nitrogen.
- the nitrogen is preferably present as pyridinic and / or quaternary nitrogen.
- Nitrogen-doped carbon nanotubes are preferably used in the inventive method as a catalytically active component of the catalyst, as obtained according to the German patent application with the application number DE 10 2007 062421.4.
- catalysts comprising nitrogen-doped carbon nanotubes as the catalytically active component in the process according to the invention is particularly advantageous because, surprisingly, in contrast to the findings of the prior art (eg US 2006/0249380), the presence of chlorine and / or chloride ions does not result in a reduction activity and thus does not result in a reduction in the oxygen reduction rate at constant, applied voltage. Furthermore, it has surprisingly been found that the nitrogen-doped carbon nanotubes are not washed out in the course of the process in chlorine- and / or chloride-containing aqueous solutions. Thus, the erf ⁇ ndungswashe method can be operated for a long time at a constant high reduction of the necessary overvoltage through the nitrogen-doped carbon nanotubes.
- a replacement of the catalytically active component is thus not necessary according to the inventive method, or only after a much longer time.
- the process according to the invention is already economically advantageous in that the use of expensive precious metals (such as, for example, platinum or rhodium) in favor of catalytically active components based on carbon modifications can be dispensed with.
- the catalysts used in the process according to the invention may also comprise catalytically active components and / or polymeric binders and / or fillers, which are generally known to the person skilled in the art. Soot.
- the catalyst used in the process according to the invention also comprises other catalytically active components well known to those skilled in the art, e.g. Rhodium sulphide or platinum.
- the catalyst used in the process according to the invention preferably comprises a polymeric binder in addition to the nitrogen-doped carbon nanotubes.
- a polymeric binder and fillers are particularly preferred.
- Polymeric binders are preferably sulfonated tetrafluoroethylene polymers (PTFE). Particularly preferred are sulfonated tetrafluoroethylene polymers, as under the name Nafion® of the Company Du Pont are sold.
- PTFE sulfonated tetrafluoroethylene polymers
- Fillers are substances which show little or no catalytic activity for the reaction according to formula (I). Suitable fillers are, for example, carbon black or graphite.
- fillers and a polymeric binder are advantageous because in the process according to the invention the catalytically active component (the nitrogen-doped carbon nanotubes or other catalytically active components known to the person skilled in the art) is present in an easily handled form or by the polymeric binder on a Fixed site and also the hydrophobicity of the catalyst can be controlled.
- the catalytically active component the nitrogen-doped carbon nanotubes or other catalytically active components known to the person skilled in the art
- the erf ⁇ ndungswashe process is usually carried out at a temperature of 0-200 0 C, preferably 30-150 0 C and particularly preferably 40-95 0 C.
- the elevated temperatures for operating the process are particularly advantageous, because in this way the reduction of oxygen can be further accelerated. It has also been found, surprisingly, that the process according to the invention has constantly high rates of reduction of oxygen even at temperatures above 60 ° C., whereas processes according to the state of the art with noble metal-containing or rhodium-sulfide-based catalytically active components at significantly higher temperatures result in a significantly faster rate Having lost the catalytically active component from the catalyst, since the solubility of the chloride salts, or chlorine complexes of the catalytically active component is increased in the aqueous solution.
- the increased pressure is advantageous because, under the elevated pressures, the solubility of the oxygen in the aqueous solution is increased under the elevated temperatures and outgassing can be prevented.
- the application of a voltage in connection with the present invention means contacting the catalyst with an electrical conductor and connecting the resulting electrode to a counter electrode via a voltage source.
- the term voltage refers to the voltage of a half cell comprising the contacted catalyst in a chlorine- and / or chloride-containing aqueous solution with respect to a normal hydrogen electrode as a reference electrode.
- the normal hydrogen electrode merely serves as a reference point for the properties of the process according to the invention with respect to the reduction of oxygen in the presence of a catalyst under stress.
- the calculation of the necessary overvoltage for the reduction of oxygen starting from the measured voltage (electrode potential) with respect to a normal hydrogen electrode is generally known to the person skilled in the art.
- the current is normalized to the geometric area of the catalyst which is in contact with the aqueous solution containing chlorine and / or chloride and denoted as the current density, expressed in kA / m 2 .
- the current density in the process according to the invention is more than 0.01 kA / m 2 , preferably between 0.1 kA / m 2 and 20 kA / m 2 , particularly preferably between 1 kA / m 2 and 10 kA / m 2 .
- the applied voltage and current density are related by laws well known to those skilled in the art, so the power to be input to the oxygen reduction process depends linearly on both parameters.
- the reduction of oxygen above a minimum necessary voltage depends only on the number of electrons transferred to oxygen, ie on the flowing current and thus on the current density.
- the voltage that must be applied in the process presented here to achieve a reduction of oxygen is comparable to that which must be applied in the prior art processes. It turns out, however, in a surprising manner that the preferred and preferred current densities according to the invention can be higher without having to fear the formation of hydrogen at the same voltage. Thus, the inventive method is safer and more economical to operate.
- the upper limits of the current densities in the preferred embodiments of the method according to the invention represent limits in the implementation of the method, since the equipment required for the representation of high current densities increases sharply and thus also increases the investment costs of devices for carrying out the erf ⁇ ndungswashen method.
- the method itself is not limited in terms of usable current densities upwards.
- a preferred further development of the process according to the invention is characterized in that the aqueous solution containing chlorine and / or chloride is formed on the catalyst by passing a gas stream comprising molecular oxygen and gaseous HCl and optionally steam over the catalyst.
- the molecular oxygen is reduced to two O 2 ions and forms water with the dissociated H ions of the HCl gas at the catalytically active component.
- the further development is advantageous because in this way the reaction is no longer influenced by a necessary diffusion of oxygen through the aqueous solution to the catalytically active component of the catalyst.
- diffusion rates in solutions are lower than in the gas phase.
- the oxygen reduction rate can be increased and the process made more economical by automatically forming only a thin aqueous film on the surface of the catalyst.
- the energy-intensive operation of pump devices for the transport and removal of aqueous solutions in connection with the preferred further development is no longer necessary. Only the gaseous starting materials of the process have to be transported to the catalyst, but not in the reduction of oxygen-inert water.
- the process according to the invention is preferably carried out as a partial process of overall chlorine production processes, so that these processes are characterized in that, in a first reaction zone in aqueous solutions containing chlorine and / or chloride, the oxygen of at least one oxygen-comprising component in the presence of a catalyst Voltage is reduced, wherein the catalyst comprises a proportion of nitrogen-doped carbon nanotubes as the catalytically active component, and in a second reaction zone chloride to chlorine is oxidized.
- Fig. 1 the change of the current density (I) as a function of the electrode potential (E) of the rotating annular disc electrode against a normal hydrogen electrode for the inventive method (A), according to Example 1, using carbon black (B), according to Example 2 and for the use of iridium catalyst (C), according to Example 3 shown.
- Example 1 Necessary voltage and current densities for oxygen reduction - process according to the invention
- a catalyst was obtained by first 40 mg of nitrogen-doped carbon nanotubes, prepared by the method according to Example 5 of the German patent application with the official file number DE 10 2007 062421.4 in 50 ml of acetone and dispersed therefrom
- the rotating annular disk electrode comprising the nitrogen-doped carbon nanotubes was used as a working electrode in a laboratory cell containing 3 electrodes (working electrode, counter electrode and reference electrode).
- the structure used is generally known to the person skilled in the art as a three-electrode arrangement.
- the electrolyte used was 5% strength by weight hydrochloric acid solution in water, which had previously been saturated with oxygen.
- the reference electrode used was an Ag / AgCl electrode. The values obtained were then related to the potential of a normal hydrogen electrode (NHE) for better comparability.
- the electrolyte was heated to 55 ° C and measurements were taken at this temperature.
- Example 2 A comparative experiment was carried out analogously to Example 1, with the only difference that carbon black (Vulcan XC72, Cabot Co.) was used instead of nitrogen-doped carbon nanotubes.
- carbon black Vulcan XC72, Cabot Co.
- Example 3 Necessary voltage and current densities for oxygen reduction - comparison with an iridium catalyst supported on Vulcan XC72
- Example 2 A comparative experiment was carried out analogously to Example 1, with the only difference that, instead of nitrogen-doped carbon nanotubes, an iridium catalyst supported on Vulcan XC72 was used.
- the iridium catalyst (20% by weight Ir) was prepared from an aqueous suspension of Vulcan XC72 (Cabot Co.) in an aqueous solution of IrCl 3 (Fluka) by precipitation with H 2 S in a basic medium (pH 10). The separated solid was calcined at 700 0 C for 2 h in a N 2 gas stream.
- Table 1 Summary of current densities and tendency to hydrogen formation
- Example 2 Experiments analogous to those in Example 1 were carried out, wherein the aqueous solution in a first experimental batch was 1 molar hydrochloric acid solution and in a second experimental batch was a 0.5 molar sulfuric acid solution. Further changes to the experimental setup compared to those in Example 1 were not made. Surprisingly, surprisingly, even in the presence of chloride ions in the aqueous solution, the process according to the invention exhibited almost the same oxygen reduction capacity as in sulfuric acid-containing medium, since the curves of both curves were almost congruent independently of the electrolyte (compare FIG. C, D, for better representability, the results of the measurements in sulfuric acid solutions were normalized to lmA / cm 2 at IV and the results of the measurements in hydrochloric acid solutions are shown relative thereto).
- Example 4 Experiments analogous to those in Example 4 were carried out using as catalyst now a rhodium-sulfide catalyst prepared according to the procedure disclosed in US 6,149,782.
- the nitrogen-doped carbon nanotubes have therefore surprisingly been shown to be very tolerant to chloride ions (Ex 4, i.V.m lines C, D of Fig. 2).
- a poisoning of the catalyst by the chloride ions and thus a significant decrease in the ability to reduce oxygen could only be found for a process comprising a rhodium-sulfide catalyst.
- Example 6 Stable operating times of the method according to the invention
- Example 2 In order to simulate a very long operating time of the method, was blended prior to an attempt to over-voltage measurement according to Example 1, the coating of the ring disk electrode for various times in 37 -% .- aqueous hydrochloric acid solution under sudfiuss at about 100 0 C treated. The treatment was carried out for one, three and five hours.
- a loss of the nitrogen content of the catalytically active component could not be detected even under the high loads, as nitrogen-doped carbon nanotubes even after five hours treatment time in 37 wt .-% aqueous hydrochloric acid solution under reflux at about 100 0 C, still above 98 % of the nitrogen originally detected prior to treatment (detected by elemental analysis, Leco®TruSpec device, method according to the manufacturer's instructions).
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Abstract
Priority Applications (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US12/922,992 US8741122B2 (en) | 2008-03-27 | 2009-03-19 | Process for the reduction of oxygen |
CN2009801108881A CN101981231A (zh) | 2008-03-27 | 2009-03-19 | 电解还原氧的方法 |
EP09725494A EP2276876A1 (fr) | 2008-03-27 | 2009-03-19 | Procédé de réduction d'oxygène électrolytique |
IL207978A IL207978A0 (en) | 2008-03-27 | 2010-09-05 | Method for the electrolytic reduction of oxygen |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE102008015902.6 | 2008-03-27 | ||
DE102008015902A DE102008015902A1 (de) | 2008-03-27 | 2008-03-27 | Verfahren zur Sauerstoffreduktion |
Publications (1)
Publication Number | Publication Date |
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WO2009118124A1 true WO2009118124A1 (fr) | 2009-10-01 |
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Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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PCT/EP2009/002028 WO2009118124A1 (fr) | 2008-03-27 | 2009-03-19 | Procédé de réduction d'oxygène électrolytique |
Country Status (7)
Country | Link |
---|---|
US (1) | US8741122B2 (fr) |
EP (1) | EP2276876A1 (fr) |
CN (1) | CN101981231A (fr) |
DE (1) | DE102008015902A1 (fr) |
IL (1) | IL207978A0 (fr) |
TW (1) | TW201006961A (fr) |
WO (1) | WO2009118124A1 (fr) |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101884932A (zh) * | 2010-06-11 | 2010-11-17 | 哈尔滨工业大学深圳研究生院 | 氮掺杂碳纳米纤维氧还原催化剂及其制备方法和应用 |
US20120279870A1 (en) * | 2009-12-18 | 2012-11-08 | Bayer Intellectual Property Gmbh | Method for electrochemical oxygen reduction in alkaline media |
Families Citing this family (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2015161310A2 (fr) * | 2014-04-18 | 2015-10-22 | The University Of North Carolina At Chapel Hill | Catalyseurs à base de nanocarbone dopé |
US20190198095A1 (en) * | 2017-12-25 | 2019-06-27 | Nanya Technology Corporation | Memory device |
US11239415B2 (en) * | 2019-04-18 | 2022-02-01 | Nanya Technology Corporation | Memory device and fabrication method thereof |
Citations (1)
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US20070275160A1 (en) * | 2003-10-10 | 2007-11-29 | Stephen Maldonado | Carbon Nanostructure-Based Electrocatalytic Electrodes |
Family Cites Families (6)
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DE19755636A1 (de) * | 1997-12-15 | 1999-06-17 | Bayer Ag | Verfahren zur elektrochemischen Aufarbeitung von HCl-Gas zu hochreinem Chlor |
US6149782A (en) | 1999-05-27 | 2000-11-21 | De Nora S.P.A | Rhodium electrocatalyst and method of preparation |
ITMI20010402A1 (it) | 2001-02-28 | 2002-08-28 | De Nora Elettrodi Spa | Nuova composizione elettrocatalitica per catodo depolarizzato ad ossigeno |
DE10335184A1 (de) | 2003-07-30 | 2005-03-03 | Bayer Materialscience Ag | Elektrochemische Zelle |
US20100314261A1 (en) * | 2005-12-14 | 2010-12-16 | Perry Michael L | Oxygen-Consuming Zero-Gap Electrolysis Cells With Porous/Solid Plates |
DE102007062421A1 (de) | 2007-12-20 | 2009-06-25 | Bayer Technology Services Gmbh | Verfahren zur Herstellung von Stickstoff-dotierten Kohlenstoffnanoröhrchen |
-
2008
- 2008-03-27 DE DE102008015902A patent/DE102008015902A1/de not_active Withdrawn
-
2009
- 2009-03-19 CN CN2009801108881A patent/CN101981231A/zh active Pending
- 2009-03-19 EP EP09725494A patent/EP2276876A1/fr not_active Withdrawn
- 2009-03-19 US US12/922,992 patent/US8741122B2/en not_active Expired - Fee Related
- 2009-03-19 WO PCT/EP2009/002028 patent/WO2009118124A1/fr active Application Filing
- 2009-03-26 TW TW098109821A patent/TW201006961A/zh unknown
-
2010
- 2010-09-05 IL IL207978A patent/IL207978A0/en unknown
Patent Citations (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20070275160A1 (en) * | 2003-10-10 | 2007-11-29 | Stephen Maldonado | Carbon Nanostructure-Based Electrocatalytic Electrodes |
Non-Patent Citations (2)
Title |
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MATTER, P.H., OZKAN, U.S.: "Non-metal catalysts for dioxygen reduction in acidic electrolyte", CATALYSIS LETTERS, vol. 109, no. 3-4, July 2006 (2006-07-01), pages 115 - 123, XP002533727 * |
ZHANG X ET AL: "A nitrogen functionalized carbon nanotube cathode for highly efficient electrocatalytic generation of H2O2 in Electro-Fenton system", SEPARATION AND PURIFICATION TECHNOLOGY, ELSEVIER SCIENCE, AMSTERDAM, NL, vol. 64, no. 1, 20 November 2008 (2008-11-20), pages 116 - 123, XP025609932, ISSN: 1383-5866, [retrieved on 20080807] * |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20120279870A1 (en) * | 2009-12-18 | 2012-11-08 | Bayer Intellectual Property Gmbh | Method for electrochemical oxygen reduction in alkaline media |
CN101884932A (zh) * | 2010-06-11 | 2010-11-17 | 哈尔滨工业大学深圳研究生院 | 氮掺杂碳纳米纤维氧还原催化剂及其制备方法和应用 |
Also Published As
Publication number | Publication date |
---|---|
TW201006961A (en) | 2010-02-16 |
DE102008015902A1 (de) | 2009-10-01 |
IL207978A0 (en) | 2010-12-30 |
US8741122B2 (en) | 2014-06-03 |
EP2276876A1 (fr) | 2011-01-26 |
US20110042231A1 (en) | 2011-02-24 |
CN101981231A (zh) | 2011-02-23 |
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